CN1434480A - Electronic device - Google Patents

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Publication number
CN1434480A
CN1434480A CN02150439A CN02150439A CN1434480A CN 1434480 A CN1434480 A CN 1434480A CN 02150439 A CN02150439 A CN 02150439A CN 02150439 A CN02150439 A CN 02150439A CN 1434480 A CN1434480 A CN 1434480A
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electrode
carbon
metal
electronic device
oxygen
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CN02150439A
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CN1319114C (en
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韩仁泽
朴永俊
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Samsung SDI Co Ltd
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Samsung SDI Co Ltd
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    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K85/00—Organic materials used in the body or electrodes of devices covered by this subclass
    • H10K85/20—Carbon compounds, e.g. carbon nanotubes or fullerenes
    • H10K85/221—Carbon nanotubes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y10/00—Nanotechnology for information processing, storage or transmission, e.g. quantum computing or single electron logic
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y30/00—Nanotechnology for materials or surface science, e.g. nanocomposites
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B82—NANOTECHNOLOGY
    • B82Y—SPECIFIC USES OR APPLICATIONS OF NANOSTRUCTURES; MEASUREMENT OR ANALYSIS OF NANOSTRUCTURES; MANUFACTURE OR TREATMENT OF NANOSTRUCTURES
    • B82Y40/00—Manufacture or treatment of nanostructures
    • C—CHEMISTRY; METALLURGY
    • C01—INORGANIC CHEMISTRY
    • C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
    • C01B32/00—Carbon; Compounds thereof
    • C01B32/15—Nano-sized carbon materials
    • C01B32/158—Carbon nanotubes
    • C01B32/16—Preparation
    • C01B32/162—Preparation characterised by catalysts
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having a potential-jump barrier or a surface barrier
    • H10K10/40—Organic transistors
    • H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
    • H10K10/462—Insulated gate field-effect transistors [IGFETs]
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K71/00—Manufacture or treatment specially adapted for the organic devices covered by this subclass
    • H10K71/60—Forming conductive regions or layers, e.g. electrodes
    • H—ELECTRICITY
    • H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
    • H10K—ORGANIC ELECTRIC SOLID-STATE DEVICES
    • H10K10/00—Organic devices specially adapted for rectifying, amplifying, oscillating or switching; Organic capacitors or resistors having a potential-jump barrier or a surface barrier
    • H10K10/40—Organic transistors
    • H10K10/46—Field-effect transistors, e.g. organic thin-film transistors [OTFT]
    • H10K10/462—Insulated gate field-effect transistors [IGFETs]
    • H10K10/466—Lateral bottom-gate IGFETs comprising only a single gate

Abstract

The present invention discloses an electronic device having an electrode made of metal that reacts easily with carbon. In the electronic device, the electrode on which carbon nanotubes are deposited by a chemical vapor deposition method using a reactant gas containing carbon and oxygen, is made of a metal generating less reaction enthalpy when reacting with carbon than when reacting with oxygen. Since the electrode is made of a metal which reacts with carbon faster than oxygen, a carbonized metal layer is formed on the electrode, thereby preventing the electrode from being oxidized. Accordingly, the carbon nanotubes can be easily deposited on the electrode.

Description

Electronic device
Technical Field
The present invention relates to an electronic device, and more particularly, to an electronic device having an electrode adapted to deposit carbon nanotubes thereon by a chemical vapor deposition method.
Background
Carbon nanotubes are used in various types of electronic devices due to their peculiar structure and electrical properties. For example, they can be used in the fields of electron emitters, hydrogen storage materials, cathode materials for secondary batteries, catalysts, and sensors. In addition, other applications of carbon nanotubes are being developed.
In the manufacture of electronic devices using carbon nanotubes, a method of using carbon nanotubes in the form of powder or slurry or a method of directly depositing carbon nanotubes on a substrate using chemical vapor deposition is used.
In a method of manufacturing an electronic device using carbon nanotube powder or paste, carbon nanotubes are subjected to laser ablation or arc discharge to obtain carbon nanotube powder, the carbon nanotube powder is mixed with conductive or non-conductive paste, and then printed.
The method using the slurry is inferior to the method using the chemical vapor deposition in terms of properties such as selective deposition or alignment. Therefore, it is expected that the method using chemical vapor deposition will be widely used for manufacturing electronic devices.
Representative chemical vapor deposition methods are thermal chemical vapor deposition methods and plasma chemical vapor deposition methods. In the aspect of low-temperature synthesis of the carbon nano tube, the plasma chemical vapor deposition method is superior to an electric field discharge method or a laser deposition method. The thermal chemical vapor deposition method is advantageous in synthesizing carbon nanotubes in a large area and in synthesizing carbon nanotubes in a large amount.
In the above chemical vapor deposition method, methane (CH)4) Acetylene (C)2H2) Or carbon monoxide (CO) is used as a reaction gas for carbon nanotube deposition.The reaction gas is mixed with, for example, hydrogen (H)2) Or ammonia (NH)3) The etching gas of (2) is mixed.
When methane is used as a reaction gas in the case of using a high-energy plasma, high-quality carbon nanotubes can be formed. When acetylene is used as the reaction gas, the carbon nanotubes can be deposited at a low temperature.
Carbon monoxide reduces the hydrogen impurity content in the carbon nanotubes, allowing high quality carbon nanotubes to be deposited at low temperatures. However, carbon monoxide is superior to oxygen atoms or groups generated during the carbon nanotube manufacturing process to chemically react with metals or other carbon molecules, thereby oxidizing the metals or generating products such as carbon dioxide. The surface of the metal that is oxidized by carbon monoxide has a reduced conductivity, which affects the accurate operation of the electronic device.
That is, when carbon monoxide, carbon dioxide (CO) are used as examples2) Methanol (CH)3OH), or ethanol (C)2H5OH) or the like is used as a reaction gas in a conventional chemical vapor deposition apparatus, the reaction gas reacts with and oxidizes a metal-formed electrode, thereby reducing the electrical conductivity of the electrode. Therefore, the performance of the electronic device is degraded.
Disclosure of Invention
In order to solve the above problems, it is an object of the present invention to provide an electronic device including an electrode, wherein conductivity of the electrode is kept constant when carbon nanotubes are deposited on the electrode using a chemical vapor deposition method, and high-quality carbon nanotubes are formed on the electrode.
In order to accomplish the above object of the present invention, in one aspect, there is provided an electronic device including an electrode on which carbon nanotubes are deposited by a chemical vapor deposition method using a reaction gas containing carbon and oxygen. The electrode is made of a metal which produces less enthalpy of reaction when reacting with carbon than when reacting with oxygen.
Preferably, the metal is one of Ti or Mo.
Preferably, the metal reacts with carbon to form a metal carbide.
The reaction gas is one of carbon monoxide, carbon dioxide, methanol and ethanol.
In another aspect, an electronic device is provided that includes an electrode on which carbon nanotubes are deposited by a chemical vapor deposition method, the electrode having a metal carbide layer formed on a surface thereof. The metal carbide layer prevents oxidation of the electrode.
Preferably, the metal is one of Ti or Mo.
Since the present invention uses a metal that generates less reaction enthalpy when reacting with carbon than when reacting with oxygen as an electrode, the metal of the electrode reacts with carbon prior to oxygen when a reaction gas containing carbon and oxygen is injected into the chemical vapor deposition apparatus, forming a metal carbide layer on the surface of the electrode. Oxygen cannot penetrate into the electrode due to the metal carbide layer. Therefore, the electrode is prevented from being oxidized, thereby maintaining the conductivity of the electrode constant and increasing the yield of the carbon nanotubes.
Drawings
The above objects and advantages of the present invention will become more apparent by describing in detail preferred embodiments thereof with reference to the attached drawings. In the drawings:
FIG. 1 is a schematic view of an electronic device having an electrode according to an embodiment of the invention;
FIG. 2 is a schematic view illustrating a method of manufacturing an electronic device having an electrode according to the embodiment of the present invention using plasma chemical vapor deposition;
FIG. 3 is a schematic view illustrating a method of fabricating an electronic device having an electrode according to the embodiment of the present invention using thermal chemical vapor deposition;
FIG. 4 is a graph of atomic concentration as a function of sputtering time after a chromium electrode is subjected to carbon nanotube deposition conditions;
FIG. 5A is a graph of atomic concentration as a function of sputtering time after an aluminum electrode is subjected to carbon nanotube deposition conditions;
FIG. 5B is a graph of counts per second (C/S) versus binding energy for an aluminum electrode under carbon nanotube deposition conditions; and
FIG. 6 is a graph of atomic concentration as a function of sputtering time after a molybdenum electrode was subjected to carbon nanotube deposition conditions.
Detailed Description
An electronic device having an electrode according to an embodiment of the present invention will be described in detail below with reference to the accompanying drawings.
FIG. 1 is a schematic view of an electronic device having an electrode according to an embodiment of the present invention. Referring to fig. 1, an insulating layer 3 is deposited on a substrate 1, twometal electrodes 5 in the form of foils are disposed to be spaced apart from each other by a predetermined distance on both sides of the surface of the insulating layer 3, and a carbon nanotube layer 7 connects the two metal electrodes 5.
This structure is the simplest current-voltage (I-V) device if the silicon is undoped, and is a Field Effect Transistor (FET) when the silicon is doped with P-type or N-type impurities.
The metal electrode 5 of the electronic device is made of a metal such as titanium (Ti) or molybdenum (Mo). The metal produces less enthalpy of reaction when reacting with carbon than with oxygen, and therefore the metal reacts with carbon at a higher rate than oxygen.
Fig. 2 is a schematic view illustrating a method of manufacturing an electronic device having an electrode according to an embodiment of the present invention using plasma chemical vapor deposition. Referring to fig. 2, in the plasma chemical vapor deposition apparatus, an upper electrode 14 and a lower electrode 12 are provided, and a substrate 11 having a catalytic metal layer formed thereon is placed on the lower electrode 12. A thermal resistive heater (thermal heater)13 located below the lower electrode 12 supplies heat to the substrate 11. The filament 15 is disposed between the upper electrode 14 and the lower electrode 12, and provides energy required for decomposition of reaction gas or synthesis of carbon nanotubes. The motor 19 rotates the lower electrode 12 on which the substrate 11 is disposed.
The metal electrode 16 of the electronic device to be manufactured is located on the surface of the catalytic metal layer on the substrate 11. The metal electrode 16 is made of a metal that generates more reaction enthalpy when reacting with carbon than when reacting with oxygen. Here, the electronic device to be manufactured may have further layers with different functions, such as an insulating layer, between the substrate 11 and the metal electrode 16.
An RF (radio frequency) power source 17 is connected to the upper electrode 14 and the lower electrode 12 to supply electric power. A pipe for injecting a reaction gas is connected at the center of the upper electrode 14 so that the reaction gas such as carbon monoxide, methane, acetylene or hydrogen is supplied to the reaction chamber 10.
When an RF power is supplied at a temperature of not more than about 660EC while maintaining a predetermined pressure after an etching gas such as ammonia or hydrogen is injected into the reaction chamber 10, the surface of the metal electrode 16 on the substrate 11 is etched by plasma generated from the etching gas, thereby forming catalytic particles in the form of fine grains on the surface of the metal electrode 16. The carbon nanotubes are synthesized and vertically arranged on the catalytic particles.
Glass, quartz, silicon or aluminium oxide (Al)2O3) A substrate may be used as the substrate 11.
The metal electrode 16 of the electronic device may be made of a metal such as Ti, Mo, or iron (Fe) that reacts with carbon at a higher rate than oxygen because it produces less reaction enthalpy when reacting with carbon than when reacting with oxygen.
Equation (1) is a chemical reaction equation showing the generation of a metal carbide upon reaction of the metal with carbon monoxide. Equation (2) is a chemical reaction equation for forming the oxidized metal.
...(1)
...(2)
In the case of Ti, the binding energy of TiO is 672.4kJ/mol, that of TiC is 423kJ/mol, the reaction enthalpy corresponding to equation (1) is-1307.1 kJ, and that corresponding to equation (2) is-808.2 kJ, thus indicating that the reaction corresponding to equation (1) is more dominant than the reaction corresponding to equation (2).
In the case of Mo, the binding energy of MoO is 560.2kJ/mol, the binding energy of MoC is 481kJ/mol, the reaction enthalpy corresponding to equation (1) is-1191 kJ, and the reaction enthalpy corresponding to equation (2) is-1032 kJ, thus indicating that the reaction corresponding to equation (1) is more dominant than the reaction corresponding to equation (2).
However, in the case of Cr, although the binding energy of CrO is 429.3kJ/mol, the binding energy of CrC is much higher than 429.3kJ/mol, and therefore, the reaction corresponding to equation (2) is more dominant than the reaction corresponding to equation (1).
Therefore, when an oxygen-containing gas such as carbon monoxide, carbon dioxide, methanol or ethanol is used as a reaction gas, a metal carbide such as titanium carbide, molybdenum carbide or iron carbide is formed on the metal surface, thereby preventing the metal from contacting oxygen.
The internal energy is reduced, resulting in negative reaction enthalpy when the chemical reaction is exothermic; the internal energy increases, resulting in a positive reaction enthalpy when the chemical reaction is endothermic. In the present invention, the chemical reaction between carbon and the metal and the chemical reaction between oxygen and the metal are exothermic reactions, and the reduction of the internal energy in the chemical reaction between carbon and the metal is larger than the reduction of the internal energy in the chemical reaction between oxygen and the metal, so the reaction enthalpy in the chemical reaction between carbon and the metal issmaller than the reaction enthalpy in the chemical reaction between oxygen and the metal. That is, more heat is generated when a metal carbide is produced by a reaction between carbon and a metal than when an oxidized metal is produced by a reaction between oxygen and a metal. Thus, it was shown that the metal carbide is more stable than the metal oxide.
Electronic devices having electrodes fabricated from metals according to embodiments of the present invention can be fabricated by thermal chemical vapor deposition methods.
Referring to fig. 3, the substrates 130 having the electrodes 110 are disposed on a boat 310 of the thermal chemical vapor deposition apparatus, the substrates are spaced apart from each other by a predetermined interval in a line, and the boat 310 is positioned in a reaction furnace 315. Thereafter, the temperature of the reaction furnace 315 is raised to a process temperature, and an etching gas and a reaction gas are injected into the reaction furnace 315 to deposit carbon nanotubes on the electrode 110.
The description of the substrate 130, the electrode 110 and the reaction gas is the same as that of the plasma chemical vapor deposition method and thus omitted.
According to the present invention, when an electronic device such as a transistor or a Field Emission Display (FED) is manufactured by a thermal chemical vapor deposition method or a plasma chemical vapor deposition method, the electrode 16 or 110 is manufactured of a metal such as Ti, Mo, or Fe that reacts faster with carbon than oxygen, and thus a metal carbide layer is formed on the electrode 16 or 110. Therefore, the electrode 16 or 110 is prevented from being oxidized during the formation of the carbon nanotube. Since the conductivity remains constant, the electronic device is easy to manufacture. Therefore, an electronic device having good performance can be manufactured.
Fig. 4 is a graph in the form of auger electron spectroscopy showing the change in atomic concentration (%) with respect to a chromium (Cr) electrode subjected to carbon nanotube fabrication using a mixed gas of carbon monoxide and hydrogen as a reaction gas.
Referring to fig. 4, as the sputtering time passes 1500 seconds, the Cr atomic concentration increases, and the oxygen (O) atomic concentration decreases. The carbon (C) atom concentration is substantially constant.
Since the chromium atom reacts with oxygen before carbon, chromium oxide (CrO) is formedx) Therefore, the Cr atomic concentration is small from the surface to a certain depth, but the concentration increases as the depth further enters the chromium electrode. On the contrary, oxygen having affinity with chromium is adsorbed more on the surface of the chromium electrode, and therefore, the concentration of O atoms is higher from the surface to a predetermined depth, and the concentration thereof decreases as the depth further penetrates into the interior of the chromium electrode. Carbon hardly reacts with chromium and therefore the C atom concentration remains almost constant.
As can be seen from the graph, chromium is more compatible with oxygen than carbon, thus indicating that chromium is not suitable as an electrode.
Fig. 5A is a graph in the form of X-ray photoelectron spectroscopy showing the change in atomic concentration with respect to an aluminum (Al) electrode that has undergone carbon nanotube fabrication using a mixed gas of carbon monoxide and hydrogen as a reaction gas.
Referring to fig. 5A, as the depth from the surface of the aluminum electrode is deeper, the Al atom concentration increases, and the O atom concentration decreases.
The aluminum reacts with oxygen or hydrogen to produce aluminum oxide (Al)2O3) Or aluminum hydride (AlH)xFor example AlH3). Referring to fig. 5, more aluminum hydride is formed as the depth from the surface of the aluminum electrode is deeper. That is, only the results shown in fig. 5A indicate that aluminum reacts mainly with oxygen to form alumina on the electrode surface; however, the graph shown in fig. 5B further indicates that aluminum hydride is more readily formed than alumina. However, aluminum hydride has a low melting point, and therefore aluminum is not suitable as an electrode.
Fig. 6 is a graph in X-ray photoelectron spectroscopy showing the change in atomic concentration with respect to a molybdenum (Mo) electrode which is included in an electronic device according to an embodiment of the present invention and has undergone carbon nanotube fabrication using a mixed gas of carbon monoxide and hydrogen as a reaction gas.
As shown in fig. 6, as the etching process proceeds, the C atom concentration decreases, while the Mo atom concentration increases, and the O atom concentration remains substantially constant. This is because the molybdenum carbide layer is formed only on the surface of the electrode and the metallic characteristics are maintained in the electrode. As can be seen from this graph, molybdenum is suitable as an electrode for use in an electronic device according to an embodiment of the present invention.
The table below shows the conductivity change for different metals. Unit is omega cm-1。
Metal Cr Mo Ti Ni Al
Before reaction 0.2 0.4 0.3 0.4 0.2
After the reaction ＞10-6 1.2 1.0 15.7 0.6
Although the conductivity of chromium is greatly reduced after undergoing the reaction in the chemical vapor deposition apparatus, the conductivity of other metals is hardly changed. As can be seen from the above table, when the electrode is made of one of four metals other than chromium, the electric power can be constantly supplied. However, aluminum sublimates in the form of aluminum hydride, and is not suitable as an electrode.
According to an embodiment of the present invention, in the case where a reaction gas containing carbon and oxygen is used in the process of forming carbon nanotubes, an electronic device has an electrode made of a metal that reacts with carbon at a higher rate than oxygen because less reaction enthalpy is generated when it reacts with carbon than when it reacts with oxygen, so that a metal carbide layer is formed on the surface of the electrode, preventing oxidation. Accordingly, the carbon nanotube can be grown on the electronic device in a state in which the conductivity of the electrode is kept constant, thereby improving the performance of the electronic device.
As described above, according to the present invention, an electronic device has an electrode made of a metal that reacts faster with carbon than oxygen, so that a metal carbide layer is formed on the electrode, thereby preventing the electrode from being oxidized. As a result, the electrical conductivity of the electrode is kept constant, thereby enabling the carbon nanotubes to be formed by various methods and improving the overall performance of the electronic device.

Claims (6)

1. An electronic device comprising an electrode on which carbon nanotubes are deposited by a chemical vapour deposition process using a reaction gas comprising carbon and oxygen, the electrode being made of a metal which producesless reaction enthalpy when reacting with carbon than when reacting with oxygen.
2. The electronic device of claim 1, wherein the metal is one of Ti and Mo.
3. The electronic device of claim 2, wherein the metal reacts with carbon to form a metal carbide.
4. The electronic device of claim 1, wherein the reactive gas is one selected from the group consisting of: carbon monoxide, carbon dioxide, methanol and ethanol.
5. An electronic device comprising an electrode on which carbon nanotubes are deposited by a chemical vapour deposition process, the electrode having a layer of metal carbide formed on its surface, the layer of metal carbide preventing oxidation of the electrode.
6. The electronic device of claim 5, wherein the metal is one of Ti and Mo.
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KR1020020003688A KR100837393B1 (en) 2002-01-22 2002-01-22 Electronic device comprising electrodes made of metal that is familiar with carbon

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CN1319114C (en) 2007-05-30
JP2003331711A (en) 2003-11-21
KR20030063530A (en) 2003-07-31
US20080152839A1 (en) 2008-06-26
KR100837393B1 (en) 2008-06-12
US20040214429A1 (en) 2004-10-28
EP1331202A3 (en) 2005-01-19
EP1331202A2 (en) 2003-07-30

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